A cation-exchange approach to tunable magnetic intercalation superlattices

Jingxuan Zhou, Jingyuan Zhou, Zhong Wan, Qi Qian, Huaying Ren, Xingxu Yan, Boxuan Zhou, Ao Zhang, Xiaoqing Pan, Wuzhang Fang, Yuan Ping, Zdenek Sofer, Yu Huang () and Xiangfeng Duan ()
Additional contact information
Jingxuan Zhou: University of California, Los Angeles
Jingyuan Zhou: University of California, Los Angeles
Zhong Wan: University of California, Los Angeles
Qi Qian: University of California, Los Angeles
Huaying Ren: University of California, Los Angeles
Xingxu Yan: University of California, Irvine
Boxuan Zhou: University of California, Los Angeles
Ao Zhang: University of California, Los Angeles
Xiaoqing Pan: University of California, Irvine
Wuzhang Fang: University of Wisconsin-Madison
Yuan Ping: University of Wisconsin-Madison
Zdenek Sofer: University of Chemistry and Technology, Prague
Yu Huang: University of California, Los Angeles
Xiangfeng Duan: University of California, Los Angeles

Nature, 2025, vol. 643, issue 8072, 683-690

Abstract: Abstract Tailoring magnetic ordering in solid-state materials is essential for emerging spintronics1,2. However, substitutional lattice doping in magnetic semiconductors is often constrained by the low solubility of magnetic elements3–5, limiting the maximum achievable doping concentration (for example, less than 5%) and ferromagnetic ordering temperature6. The intercalation of magnetic elements in layered two-dimensional atomic crystals (2DACs) without breaking in-plane covalent bonds offers an alternative approach to incorporate a much higher concentration of magnetic atoms (for example, up to 50%) beyond the typical solubility limit. However, commonly used chemical and electrochemical intercalation methods are largely confined to a few isolated examples so far. Here we report a general two-step intercalation and cation-exchange strategy to produce a library of highly ordered magnetic intercalation superlattices (MISLs) with tunable magnetic ordering. Monovalent transition-metal cations Cu+ and Ag+, divalent magnetic cations Mn2+, Fe2+, Co2+ and Ni2+, and trivalent rare-earth cations Eu3+ and Gd3+ have been successfully incorporated into group-VIB 2DACs, including MoS2, MoSe2, MoTe2, WS2, WSe2 and WTe2, and group-IVB, -VB, -IIIA, -IVA and -VA 2DACs, including TiS2, NbS2, NbSe2, TaS2, In2Se3, SnSe2, Bi2Se3 and Bi2Te3. We show that these MISLs can be prepared with tunable concentrations of magnetic intercalants, enabling tailored magnetic ordering across a diverse array of functional 2DACs, including semiconductors, topological insulators, and superconductors. This work establishes a versatile material platform for both fundamental investigations and spintronics applications.

Date: 2025
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DOI: 10.1038/s41586-025-09147-z

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